Metal-Free Boron/Phosphorus Co-Doped Nanoporous Carbon for Highly Efficient Benzyl Alcohol Oxidation

被引:32
作者
Meng, Juan [1 ]
Tong, Zhihan [1 ]
Sun, Haixin [1 ]
Liu, Yongzhuang [1 ]
Zeng, Suqing [1 ]
Xu, Jianing [1 ]
Xia, Qinqin [1 ]
Pan, Qingjiang [2 ]
Dou, Shuo [1 ]
Yu, Haipeng [1 ]
机构
[1] Northeast Forestry Univ, Key Lab Biobased Mat Sci & Technol, Minist Educ, Harbin 150040, Peoples R China
[2] Heilongjiang Univ, Sch Chem & Mat Sci, Key Lab Funct Inorgan Mat Chem, Harbin 150080, Peoples R China
关键词
alcohol oxidation; boron; carbon; cellulose; codoping; metal-free catalysts; SINGLE-ATOM CATALYSTS; AEROBIC OXIDATION; OXYGEN REDUCTION; GRAPHENE; PERFORMANCE; PHOSPHORUS; DESCRIPTOR; NANOSHEETS; NANOTUBES; ENERGY;
D O I
10.1002/advs.202200518
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
An in-depth understanding of the electronic structures of catalytically active centers and their surrounding vicinity is key to clarifying the structure-activity relationship, and thus enabling the design and development of novel metal-free carbon-based materials with desired catalytic performance. In this study, boron atoms are introduced into phosphorus-doped nanoporous carbon via an efficient strategy, so that the resulting material delivers better catalytic performance. The doped B atoms alter the electronic structures of active sites and cause the adjacent C atoms to act as additional active sites that catalyze the reaction. The B/P co-doped nanoporous carbon shows remarkable catalytic performance for benzyl alcohol oxidation, achieving high yield (over 91% within 2 h) and selectivity (95%), as well as low activation energy (32.2 kJ mol(-1)). Moreover, both the conversion and selectivity remain above 90% after five reaction cycles. Density functional theory calculations indicate that the introduction of B to P-doped nanoporous carbon significantly increases the electron density at the Fermi level and that the oxidation of benzyl alcohol occurs via a different reaction pathway with a very low energy barrier. These findings provide important insights into the relationship between catalytic performance and electronic structure for the design of dual-doped metal-free carbon catalysts.
引用
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页数:10
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